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Title: Strongly correlated perovskite lithium ion shuttles

Abstract

Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and biomimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO 3 (Li-SNO) contains a large amount of mobile Li + located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li + conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na + . The results highlight the potential of quantum materials and emergent physics in design of ion conductors.

Authors:
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Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1464333
Alternate Identifier(s):
OSTI ID: 1482565; OSTI ID: 1493889
Report Number(s):
BNL-209464-2018-JAAM
Journal ID: ISSN 0027-8424; /pnas/115/39/9672.atom
Grant/Contract Number:  
SC0012704; AC02-06CH11357; AC02-05CH1123
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 39; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ionic conductivity; emergent phenomena; Mott transition; neuromorphic; perovskite nickelate

Citation Formats

Sun, Yifei, Kotiuga, Michele, Lim, Dawgen, Narayanan, Badri, Cherukara, Mathew, Zhang, Zhen, Dong, Yongqi, Kou, Ronghui, Sun, Cheng-Jun, Lu, Qiyang, Waluyo, Iradwikanari, Hunt, Adrian, Tanaka, Hidekazu, Hattori, Azusa N., Gamage, Sampath, Abate, Yohannes, Pol, Vilas G., Zhou, Hua, Sankaranarayanan, Subramanian K. R. S., Yildiz, Bilge, Rabe, Karin M., and Ramanathan, Shriram. Strongly correlated perovskite lithium ion shuttles. United States: N. p., 2018. Web. doi:10.1073/pnas.1805029115.
Sun, Yifei, Kotiuga, Michele, Lim, Dawgen, Narayanan, Badri, Cherukara, Mathew, Zhang, Zhen, Dong, Yongqi, Kou, Ronghui, Sun, Cheng-Jun, Lu, Qiyang, Waluyo, Iradwikanari, Hunt, Adrian, Tanaka, Hidekazu, Hattori, Azusa N., Gamage, Sampath, Abate, Yohannes, Pol, Vilas G., Zhou, Hua, Sankaranarayanan, Subramanian K. R. S., Yildiz, Bilge, Rabe, Karin M., & Ramanathan, Shriram. Strongly correlated perovskite lithium ion shuttles. United States. doi:10.1073/pnas.1805029115.
Sun, Yifei, Kotiuga, Michele, Lim, Dawgen, Narayanan, Badri, Cherukara, Mathew, Zhang, Zhen, Dong, Yongqi, Kou, Ronghui, Sun, Cheng-Jun, Lu, Qiyang, Waluyo, Iradwikanari, Hunt, Adrian, Tanaka, Hidekazu, Hattori, Azusa N., Gamage, Sampath, Abate, Yohannes, Pol, Vilas G., Zhou, Hua, Sankaranarayanan, Subramanian K. R. S., Yildiz, Bilge, Rabe, Karin M., and Ramanathan, Shriram. Mon . "Strongly correlated perovskite lithium ion shuttles". United States. doi:10.1073/pnas.1805029115.
@article{osti_1464333,
title = {Strongly correlated perovskite lithium ion shuttles},
author = {Sun, Yifei and Kotiuga, Michele and Lim, Dawgen and Narayanan, Badri and Cherukara, Mathew and Zhang, Zhen and Dong, Yongqi and Kou, Ronghui and Sun, Cheng-Jun and Lu, Qiyang and Waluyo, Iradwikanari and Hunt, Adrian and Tanaka, Hidekazu and Hattori, Azusa N. and Gamage, Sampath and Abate, Yohannes and Pol, Vilas G. and Zhou, Hua and Sankaranarayanan, Subramanian K. R. S. and Yildiz, Bilge and Rabe, Karin M. and Ramanathan, Shriram},
abstractNote = {Solid-state ion shuttles are of broad interest in electrochemical devices, nonvolatile memory, neuromorphic computing, and biomimicry utilizing synthetic membranes. Traditional design approaches are primarily based on substitutional doping of dissimilar valent cations in a solid lattice, which has inherent limits on dopant concentration and thereby ionic conductivity. Here, we demonstrate perovskite nickelates as Li-ion shuttles with simultaneous suppression of electronic transport via Mott transition. Electrochemically lithiated SmNiO 3 (Li-SNO) contains a large amount of mobile Li + located in interstitial sites of the perovskite approaching one dopant ion per unit cell. A significant lattice expansion associated with interstitial doping allows for fast Li + conduction with reduced activation energy. We further present a generalization of this approach with results on other rare-earth perovskite nickelates as well as dopants such as Na + . The results highlight the potential of quantum materials and emergent physics in design of ion conductors.},
doi = {10.1073/pnas.1805029115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 39,
volume = 115,
place = {United States},
year = {2018},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1805029115

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Cited by: 4 works
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